Engineering hybrid nanotube wires for high-power biofuel cells.

Poor electron transfer and slow mass transport of substrates are significant rate-limiting steps in electrochemical systems. It is especially true in biological media, in which the concentrations and diffusion coefficients of substrates are low, hindering the development of power systems for miniaturized biomedical devices. In this study, we show that the newly engineered porous microwires comprised of assembled and oriented carbon nanotubes (CNTs) overcome the limitations of small dimensions and large specific surface area. Their improved performances are shown by comparing the electroreduction of oxygen to water in saline buffer on carbon and CNT fibres. Under air, and after several hours of operation, we show that CNT microwires exhibit more than tenfold higher performances than conventional carbon fibres. Consequently, under physiological conditions, the maximum power density of a miniature membraneless glucose/oxygen CNT biofuel cell exceeds by far the power density obtained for the current state of art carbon fibre biofuel cells.

[1]  Allen J. Bard,et al.  Electrochemical Methods: Fundamentals and Applications , 1980 .

[2]  Adam Heller,et al.  Electrical Wiring of Redox Enzymes , 1990 .

[3]  Adam Heller,et al.  Electrical Connection of Enzyme Redox Centers to Electrodes , 1992 .

[4]  P. Poulin,et al.  Macroscopic fibers and ribbons of oriented carbon nanotubes. , 2000, Science.

[5]  Adam Heller,et al.  Mechanical and Electrochemical Characteristics of Composites of Wired Glucose Oxidase and Hydrophilic Graphite , 2000 .

[6]  A Heller,et al.  A miniature biofuel cell. , 2001, Journal of the American Chemical Society.

[7]  Patrick Bernier,et al.  Macroscopic Fibers and Ribbons of Oriented Carbon Nanotubes. , 2001 .

[8]  W. D. de Heer,et al.  Carbon Nanotubes--the Route Toward Applications , 2002, Science.

[9]  Shoushan Fan,et al.  Nanotechnology: Spinning continuous carbon nanotube yarns , 2002, Nature.

[10]  Adam Heller,et al.  A miniature biofuel cell operating in a physiological buffer. , 2002, Journal of the American Chemical Society.

[11]  Adam Heller,et al.  An oxygen cathode operating in a physiological solution. , 2002, Journal of the American Chemical Society.

[12]  Adam Heller,et al.  On the relationship between the characteristics of bilirubin oxidases and O2 cathodes based on their wiring , 2002 .

[13]  N. Mano,et al.  Characteristics of a miniature compartment-less glucose-O2 biofuel cell and its operation in a living plant. , 2003, Journal of the American Chemical Society.

[14]  M. Maugey,et al.  Hierarchical Pore Structure and Wetting Properties of Single-Wall Carbon Nanotube Fibers , 2003 .

[15]  José L. Fernández,et al.  Oxygen is electroreduced to water on a "wired" enzyme electrode at a lesser overpotential than on platinum. , 2003, Journal of the American Chemical Society.

[16]  Adam Heller,et al.  Long tethers binding redox centers to polymer backbones enhance electron transport in enzyme "Wiring" hydrogels. , 2003, Journal of the American Chemical Society.

[17]  Scott Calabrese Barton,et al.  Enzymatic biofuel cells for implantable and micro-scale devices , 2004 .

[18]  Myung Jong Kim,et al.  Macroscopic, Neat, Single-Walled Carbon Nanotube Fibers , 2002, Science.

[19]  A. Heller Miniature biofuel cells , 2004 .

[20]  Pedro Gómez-Romero,et al.  Functional Hybrid Materials , 2004 .

[21]  Adam Heller,et al.  A four-electron O(2)-electroreduction biocatalyst superior to platinum and a biofuel cell operating at 0.88 V. , 2004, Journal of the American Chemical Society.

[22]  K. R. Atkinson,et al.  Multifunctional Carbon Nanotube Yarns by Downsizing an Ancient Technology , 2004, Science.

[23]  Electrochemistry of Sol‐Gel Derived Hybrid Materials , 2005 .

[24]  G. Wallace,et al.  Carbon nanotube based electronic and electrochemical sensors , 2005 .

[25]  J. Justin Gooding,et al.  Nanostructuring electrodes with carbon nanotubes: A review on electrochemistry and applications for sensing , 2005 .

[26]  Joseph Wang Carbon‐Nanotube Based Electrochemical Biosensors: A Review , 2005 .

[27]  Wei Zheng,et al.  Direct Electrochemistry of Multi-Copper Oxidases at Carbon Nanotubes Noncovalently Functionalized with Cellulose Derivatives , 2006 .

[28]  Wei Zheng,et al.  Carbon‐Nanotube‐Based Glucose/O2 Biofuel Cells , 2006 .

[29]  Jerzy P. Łukaszewicz,et al.  Carbon Materials for Chemical Sensors: A Review , 2006 .

[30]  Marek Trojanowicz,et al.  Analytical applications of carbon nanotubes : a review , 2006 .

[31]  Frédéric Barrière,et al.  A laccase-glucose oxidase biofuel cell prototype operating in a physiological buffer , 2006 .

[32]  A Laccase-Glucose Oxidase Biofuel Cell Prototype , 2006 .

[33]  Adam Heller,et al.  A laccase-wiring redox hydrogel for efficient catalysis of O2 electroreduction. , 2006, The journal of physical chemistry. B.

[34]  E. Bekyarova,et al.  Functionalized Single-Walled Carbon Nanotubes for Carbon Fiber−Epoxy Composites† , 2007 .

[35]  Feng Gao,et al.  An enzymatic glucose/O2 biofuel cell: Preparation, characterization and performance in serum , 2007 .

[36]  K. Seshan,et al.  Preparation and Application of Carbon-Nanofiber Based Microstructured Materials as Catalyst Supports , 2007 .

[37]  Michael Sennett,et al.  High-Performance Carbon Nanotube Fiber , 2007, Science.

[38]  Geoffrey M. Spinks,et al.  A novel dual mode actuation in chitosan/ polyaniline/carbon nanotube fibers , 2007 .

[39]  L. Mao,et al.  Multi-walled carbon nanotube-based glucose/O2 biofuel cell with glucose oxidase and laccase as biocatalysts. , 2007, Journal of nanoscience and nanotechnology.

[40]  J. Hone,et al.  Mediated Enzyme Electrodes with Combined Micro- and Nanoscale Supports , 2007 .

[41]  Bor Yann Liaw,et al.  Enzyme-based biofuel cells. , 2007, Current opinion in biotechnology.

[42]  N. Mano,et al.  On the behavior of the porous rotating disk electrode , 2007 .

[43]  I. Willner,et al.  Integrated, electrically contacted NAD(P)+-dependent enzyme-carbon nanotube electrodes for biosensors and biofuel cell applications. , 2007, Chemistry.

[44]  Luke Roberson,et al.  Solid-state spun fibers and yarns from 1-mm long carbon nanotube forests synthesized by water-assisted chemical vapor deposition , 2008 .

[45]  Vojtech Svoboda,et al.  Enzyme catalysed biofuel cells , 2008 .

[46]  S. Tingry,et al.  Concentric glucose/O2 biofuel cell , 2008 .

[47]  T. Ohsaka,et al.  A Miniature glucose/O2 biofuel cell with single-walled carbon nanotubes-modified carbon fiber microelectrodes as the substrate , 2008 .

[48]  F. Armstrong,et al.  Enzymes as working or inspirational electrocatalysts for fuel cells and electrolysis. , 2008, Chemical reviews.

[49]  Maria Forsyth,et al.  High Rates of Oxygen Reduction over a Vapor Phase–Polymerized PEDOT Electrode , 2008, Science.

[50]  Itamar Willner,et al.  Integrated Enzyme‐Based Biofuel Cells–A Review , 2009 .

[51]  Christopher P. Rhodes,et al.  Development of a biofuel cell using glucose-oxidase- and bilirubin-oxidase-based electrodes , 2009 .

[52]  Evgeny Katz,et al.  Biofuel cell controlled by enzyme logic systems. , 2009, Journal of the American Chemical Society.

[53]  F. Gao,et al.  Deglycosylation of glucose oxidase for direct and efficient glucose electrooxidation on a glassy carbon electrode. , 2009, Angewandte Chemie.

[54]  Taiki Sugiyama,et al.  A High-Power Glucose/Oxygen Biofuel Cell Operating under Quiescent Conditions , 2009, ECS Transactions.

[55]  F. Du,et al.  Nitrogen-Doped Carbon Nanotube Arrays with High Electrocatalytic Activity for Oxygen Reduction , 2009, Science.